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Title: Feasibility of Valence-to-Core X-ray Emission Spectroscopy for Tracking Transient Species

X-ray spectroscopies, when combined in laser-pump, X-ray-probe measurement schemes, can be powerful tools for tracking the electronic and geometric structural changes that occur during the course of a photoinitiated chemical reaction. X-ray absorption spectroscopy (XAS) is considered an established technique for such measurements, and X-ray emission spectroscopy (XES) of the strongest core-to-core emission lines (Kα and Kβ) is now being utilized. Flux demanding valence-to-core XES promises to be an important addition to the time-resolved spectroscopic toolkit. Here In this paper we present measurements and density functional theory calculations on laser-excited, solution-phase ferrocyanide that demonstrate the feasibility of valence-to-core XES for time-resolved experiments. Lastly, we discuss technical improvements that will make valence-to-core XES a practical pump–probe technique.
Authors:
 [1] ;  [2] ;  [3] ;  [1] ;  [2] ;  [2] ;  [1] ;  [4] ;  [4] ;  [1] ;  [1] ;  [4]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). X-ray Science Division
  2. European x-ray free electron laser (XFEL), Hamburg (Germany)
  3. European x-ray free electron laser (XFEL), Hamburg (Germany); Hamburg Centre for Ultrafast Imaging, Hamburg (Germany)
  4. Hungarian Academy Sciences, Budapest (Hungary). Wigner Research Centre for Physics
Publication Date:
OSTI Identifier:
1225106
Grant/Contract Number:
ERC-tG-259709; SFB925; AC02-06CH11357
Type:
Published Article
Journal Name:
Journal of Physical Chemistry. C
Additional Journal Information:
Journal Volume: 119; Journal Issue: 26; Journal ID: ISSN 1932-7447
Publisher:
American Chemical Society
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); European Research Council (ERC)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY